Journal of Colloid and Interface Science最新文献_第10页

Microneedle-mediated transdermal delivery of cerium‑iron bimetallic organic frameworks derivatives for melanoma therapy: enhanced peroxidase-like activity and adenosine triphosphate hydrolysis effect 微针介导的经皮递送铈-铁双金属有机框架衍生物用于黑色素瘤治疗：增强过氧化物酶样活性和三磷酸腺苷水解作用。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-01 Epub Date: 2026-01-12 DOI: 10.1016/j.jcis.2026.139885

Panpan Huo , Linghuan Guo , Haifeng Zhang , Shiwei Guan , Shun Xing , Sicong Chen , Haobo Pan , Lidan Liu , Xuanyong Liu

Cutaneous melanoma is highly metastatic and deadly, with conventional therapies often proving ineffective while causing significant side effects. Cerium-based metal-organic frameworks (Ce-MOFs) and their derivatives have recently attracted attention in antitumor therapy due to their unique physicochemical properties and multi-enzyme-mimicking activities. However, their catalytic efficiency remains suboptimal because of challenges such as ambiguous active sites and low utilization efficiency of metal ions. Their therapeutic efficacy is also frequently hampered by inefficient delivery systems. Here, a microneedle (MN) patch-assisted transdermal delivery system of oxygen vacancy-rich cerium‑iron bimetallic organic framework (CeFe-MOFs) derivatives (CeFeO_x) is constructed for synergistic chemodynamic (CDT) and starvation therapy against melanoma. Compared with Ce-MOFs derivatives (CeO_x), CeFeO_x exhibits superior peroxidase-like (POD-like) activity, which may be attributed to Fe doping increasing the Ce³⁺/Ce⁴⁺ ratio and, consequently, the concentration of oxygen vacancies. Through theoretical calculations, the catalytic pathway of CeFeO_x toward H₂O₂ and the mechanism by which Fe doping enhances the POD-like activity of CeO_x are further revealed. The results indicate that the enhanced POD-like activity of CeFeO_x originates from local changes in the electronic structure of the cerium lattice induced by Fe doping, which reduces the activation energy of key reaction steps. Meanwhile, Fe doping promotes the adenosine triphosphate (ATP) hydrolysis ability of CeO_x, which is attributed to the strong binding affinity between Fe³⁺ and ATP. The MN patch penetrates the stratum corneum, enabling efficient delivery of CeFeO_x to intratumoral regions and thereby inducing melanoma cell death. Taken together, the MN-assisted cutaneous delivery system of CeFeO_x provides a reasonable strategy for treating melanoma with highly enhanced catalytic activity.

皮肤黑色素瘤是高度转移和致命的，传统的治疗方法往往被证明是无效的，而且会引起明显的副作用。铈基金属有机骨架（Ce-MOFs）及其衍生物由于其独特的物理化学性质和多酶模拟活性，近年来在抗肿瘤治疗中受到广泛关注。然而，由于活性位点不明确和金属离子利用率低等挑战，它们的催化效率仍然不是最佳的。它们的治疗效果也经常受到低效的输送系统的阻碍。本文构建了一种微针（MN）贴片辅助的富氧铈-铁双金属有机骨架（CeFe-MOFs）衍生物（CeFeOx）透皮给药系统，用于协同化学动力学（CDT）和饥饿治疗黑色素瘤。与CeOx相比，CeFeOx表现出更强的过氧化物酶活性，这可能是由于Fe掺杂增加了Ce3+/Ce4+的比例，从而增加了氧空位的浓度。通过理论计算，进一步揭示了CeFeOx对H2O2的催化途径以及Fe掺杂增强CeFeOx类pod活性的机理。结果表明，CeFeOx的pod样活性增强源于Fe掺杂引起的铈晶格电子结构的局部变化，降低了关键反应步骤的活化能。同时，Fe掺杂促进了CeOx对三磷酸腺苷（adenosine triphosphate， ATP）的水解能力，这是由于Fe3+与ATP之间具有很强的结合亲和力。MN贴片穿透角质层，使CeFeOx能够有效地递送到瘤内区域，从而诱导黑色素瘤细胞死亡。综上所述，mn辅助的CeFeOx皮肤递送系统为治疗黑色素瘤提供了一种合理的策略，具有高度增强的催化活性。

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引用次数: 0

Surface and interfacial engineering of P2-type layered oxides through Li/Mg/Si tri-doping toward stable and fast sodium-ion transport Li/Mg/Si三掺杂p2型层状氧化物的表面和界面工程，以实现稳定和快速的钠离子输运。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-01 Epub Date: 2026-01-12 DOI: 10.1016/j.jcis.2026.139875

Chunlin Chi , Fan Liu , Shuai Jiang , Taoliang Zhou , Dawei Chen , Yujue Wang , Bin He , Qian Zhao

Interfacial engineering is a decisive factor in stabilizing layered oxide cathodes for sodium-ion batteries (SIBs). Here, a synergistic Li/Mg/Si tri-doping strategy is introduced to simultaneously modulate the bulk lattice and interfacial chemistry of a P2-type Na_0.7Li_0.03Mg_0.05Ni_0.25Mn_{0. 6}Si_0.07O₂ (LMNMS) cathode. The dopants expand the c-axis lattice (11.195 Å) and strengthen surface transition metal (TM)-O covalency, yielding improved Na⁺ diffusion kinetics and interfacial stability. X-ray photoelectron spectroscopy (XPS) and in situ Raman analyses reveal reduced surface oxygen vacancies (15% vs. 22% in the undoped sample) and suppressed electrolyte-induced oxygen redox, effectively mitigating the P2 → O2 phase transition. Electrochemical impedance spectroscopy confirms a 45% decrease in charge-transfer resistance, indicating enhanced interfacial charge transport. Benefiting from this coupled bulk-surface optimization, LMNMS delivers a high reversible capacity of 165 ± 3.2 mAh g⁻¹ at 0.1C, an excellent rate performance (92 ± 2.5 mAh g⁻¹ at 5C), and 90.5 ± 1.8% capacity retention after 200 cycles. This work highlights how multi-site doping tailors both the electronic and chemical nature of electrode interfaces, offering a design paradigm for high-performance and interface-stable sodium-ion batteries.

界面工程是稳定钠离子电池层状氧化物阴极的决定性因素。本文采用Li/Mg/Si三掺杂策略，同时调控了p2型Na0.7Li0.03Mg0.05Ni0.25Mn0的体晶格和界面化学性质。6Si0.07O2 （LMNMS）阴极。掺杂剂扩展了c轴晶格（11.195 Å），增强了表面过渡金属(TM)-O共价，提高了Na+扩散动力学和界面稳定性。x射线光电子能谱（XPS）和原位拉曼分析显示，表面氧空位减少（15% vs. 22%），电解质诱导的氧氧化还原被抑制，有效地减缓了P2→O2相变。电化学阻抗谱证实电荷传递电阻降低了45%，表明界面电荷传输增强。得益于这种耦合体-表面优化，LMNMS在0.1C时具有165±3.2 mAh g-1的高可逆容量，在5C时具有92±2.5 mAh g-1的优异倍率性能，200次循环后的容量保持率为90.5±1.8%。这项工作强调了多位点掺杂如何调整电极界面的电子和化学性质，为高性能和界面稳定的钠离子电池提供了一种设计范例。

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引用次数: 0

A unique approach to significantly enhance the emission intensity of Cr3+ via reverse defect energy level control method 采用逆向缺陷能级控制方法显著提高Cr3+的发射强度。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-01 Epub Date: 2026-01-19 DOI: 10.1016/j.jcis.2026.139928

Chengyu Cai , Chuang Wang , Nana Jia , Cheng Gong , Jianhao Li , Xiaoyi Liu , Ge Zhu

In recent years, Cr³⁺ doped near-infrared (NIR) phosphors have garnered significant scholarly interest due to their distinct properties and diverse applications. Nevertheless, the coexistence of Cr³⁺ and Cr⁴⁺ ions significantly impinges on luminous intensity and NIR efficiency. Here, for the first time, we propose a reverse defect energy level control method to enhance the emission intensity of Cr³⁺ by blocking the energy transfer pathway from Cr³⁺ to Cr⁴⁺. By doping Sr²⁺ ions in Ba₉Sc₂Si₆O₂₄:Cr³⁺/Cr⁴⁺, the luminescence intensity increased by 10 times, and the quantum efficiency rose from 2.9% to 25.6%. The full width at half maximum (FWHM) simultaneously decreased from 461 nm to 180 nm, setting a record. The defect energy level control method of inhibiting energy transfer could be conclusively demonstrated through luminescence kinetics testing, TL spectrum analysis, and associated theoretical calculations. Through precise defect regulation, the energy transfer efficiency between Cr³⁺ and Cr⁴⁺ decreased from 76.85% to 0%. The NIR pc-LEDs were synthesized by integrating the developed phosphor with a commercial 460 nm blue chip, exhibiting a photoelectric efficiency of 8.5% at 100 mA and a NIR output power of 28 mW at 100 mA. By spin-coating with Ba_8.28Sr_0.72Sc₂Si₆O₂₄:0.01Cr³⁺ phosphor, the relative conversion efficiency of the c-Si solar cell is increased by 31.2% compared to the bare c-Si solar cell. Furthermore, this work presents a novel insight to enhance the luminescence intensity of Cr³⁺ by inhibiting energy transfer in the coexistence system of Cr³⁺ and Cr⁴⁺.

近年来，Cr3+掺杂近红外（NIR）荧光粉由于其独特的性质和多样化的应用而引起了极大的学术兴趣。然而，Cr3+和Cr4+离子的共存对发光强度和近红外效率有显著影响。本文首次提出了一种反向缺陷能级控制方法，通过阻断Cr3+到Cr4+的能量传递途径来增强Cr3+的发射强度。在Ba9Sc2Si6O24:Cr3+/Cr4+中掺杂Sr2+离子，发光强度提高了10倍，量子效率从2.9%提高到25.6%。半最大全宽度（FWHM）同时从461 nm减少到180 nm，创下了记录。通过发光动力学测试、TL光谱分析和相关理论计算，最终证明了抑制能量转移的缺陷能级控制方法。通过精确的缺陷调节，Cr3+和Cr4+之间的能量传递效率从76.85%降低到0%。将所制备的荧光粉与商用460 nm蓝色芯片集成，合成了近红外pc- led，在100 mA时光电效率为8.5%，在100 mA时近红外输出功率为28 mW。采用Ba8.28Sr0.72Sc2Si6O24:0.01Cr3+荧光粉自旋镀膜后，c-Si太阳电池的相对转换效率比裸c-Si太阳电池提高了31.2%。此外，本工作还提出了通过抑制Cr3+和Cr4+共存体系中的能量转移来增强Cr3+发光强度的新见解。

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引用次数: 0

Bifunctional Li4SiO4 nanowires via one-pot synthesis for low-concentration CO2 capture and thermochemical energy storage 一锅合成双功能Li4SiO4纳米线用于低浓度CO2捕获和热化学储能。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-01 Epub Date: 2026-01-20 DOI: 10.1016/j.jcis.2026.139945

Shuo Chen , Chuanzhou Geng , Shikun Wen , Enju Zhu , Daoping Zhan , Ping Ning , Yu Zhang , Junya Wang

The practical application of lithium silicate (Li₄SiO₄) in high-temperature CO₂ capture is limited by its deteriorated sorption performance under low-concentration CO₂ atmospheres and poor long-term cycling stability. Additionally, its inherent powder form poses significant challenges for industrial implementation. Meanwhile, as a thermochemical energy storage material, its stability is equally crucial. To address these issues, this study developed a novel Li₄SiO₄ sorbent featuring nanowire-like Li₄SiO₄ crystallites on the particle surface by utilizing mixed lithium sources (LiOH/LiNO₃) and pumice (PU). The synthesized Li₄SiO₄ not only retains the porous granular structure of pumice but also exhibits excellent sorption performance and regeneration stability under low CO₂ concentrations. The results demonstrate that when the molar ratio of LiOH/LiNO₃ is 7:3, the synthesized Li₄SiO₄ particles (PU-Li₄SiO₄–0.7LH/0.3LN) exhibit nanowire-like Li₄SiO₄ crystallites on the particle surface. Under conditions of 600 °C and 20 vol% CO₂ concentration, it achieves a sorption capacity of 29.5 wt% and a thermochemical storage capacity of 629.2 kJ/kg, significantly surpassing pure Li₄SiO₄. Moreover, PU-Li₄SiO₄–0.7LH/0.3LN demonstrates remarkable sorption-regeneration stability. After 150 cycles of reaction at 20 vol% CO₂ concentration, the sorption capacity of PU-Li₄SiO₄–0.7LH/0.3LN decreased only from 21.4 wt% to 19.9 wt%. This excellent performance is attributed not only to the nanowire-like Li₄SiO₄ crystallites providing abundant sorption sites, but also to the natural porous structure of pumice offering stable gas transport channels.

硅酸锂（Li4SiO4）在低浓度CO2环境下的吸附性能变差，长期循环稳定性差，限制了其在高温CO2捕集中的实际应用。此外，其固有的粉末形式对工业实施提出了重大挑战。同时，作为一种热化学储能材料，其稳定性同样至关重要。为了解决这些问题，本研究利用混合锂源（LiOH/LiNO3）和浮石（PU）开发了一种新型的Li4SiO4吸附剂，其颗粒表面具有纳米线状的Li4SiO4晶体。合成的Li4SiO4不仅保留了浮石的多孔颗粒结构，而且在低CO2浓度下表现出优异的吸附性能和再生稳定性。结果表明：当LiOH/LiNO3的摩尔比为7:3时，合成的Li4SiO4颗粒（PU-Li4SiO4-0.7LH/0.3LN）表面呈现纳米线状的Li4SiO4晶体；在600°C和20 vol% CO2浓度条件下，其吸附容量为29.5 wt%，热化学储存容量为629.2 kJ/kg，明显优于纯Li4SiO4。此外，PU-Li4SiO4-0.7LH/0.3LN具有显著的吸附再生稳定性。在20 vol% CO2浓度下反应150次后，PU-Li4SiO4-0.7LH/0.3LN的吸附量仅从21.4% wt%下降到19.9% wt%。这种优异的性能不仅归功于纳米线状的Li4SiO4晶体提供了丰富的吸附位点，而且浮石的天然多孔结构提供了稳定的气体输送通道。

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引用次数: 0

Ethanol-mediated electrochemical reconstruction for efficient catalysts for oxygen evolution reaction 乙醇介导的析氧反应高效催化剂的电化学重构

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-01 Epub Date: 2026-01-20 DOI: 10.1016/j.jcis.2026.139950

Xiaotong Mao , Mingjuan Zhang , Ya Tang , Hongzhan Chen , Lijie Zhu , Wenyu Huang , Fangyan Xie , Jian Chen , Nan Wang , Yanshuo Jin , Hui Meng

Developing efficient and durable oxygen evolution reaction (OER) catalysts is of great significance for achieving industrial-scale production of green hydrogen. This study proposes an innovative ethanol-mediated electrochemical surface reconstruction strategy to significantly enhance the OER activity of nickel-based catalysts. This strategy effectively promotes the transformation of Ni(OH)₂ into the highly active γ-NiOOH phase, which greatly increases the density of surface Ni³⁺ active sites and optimizes the catalyst's microstructure and electronic properties. After electrochemical reconstruction, the Ni(OH)₂-R exhibits outstanding catalytic activity, requiring an overpotential of only 270 mV at 100 mA cm⁻². This represents a substantial reduction of 155 mV compared to the untreated sample. This strategy is also successfully applied to Mo-doped Ni(OH)₂ and commercial nickel mesh (NiAl-NM). Furthermore, the catalyst activity can be regenerated through simple electrolyte replacement and short-term reconstruction treatment after long-term operation, thereby extending catalyst's service life. This work presents promising prospects for industrial applications due to its simple process, low cost, and capability for in situ activity regeneration, which holds significant implications for advancing water electrolysis hydrogen production technology.

开发高效、耐用的析氧反应催化剂对实现绿色氢的工业化生产具有重要意义。本研究提出了一种创新的乙醇介导的电化学表面重构策略，以显著提高镍基催化剂的OER活性。该策略有效地促进了Ni(OH)2向高活性的γ-NiOOH相转变，大大增加了表面Ni3+活性位点的密度，优化了催化剂的微观结构和电子性能。电化学重构后，Ni(OH)2- r表现出优异的催化活性，在100 mA cm−2下，过电位仅为270 mV。与未经处理的样品相比，这代表了155 mV的大幅降低。该策略也成功应用于mo掺杂Ni(OH)2和商用镍网（NiAl-NM）。此外，在长期使用后，通过简单的电解液更换和短期的重建处理，可以使催化剂活性再生，从而延长催化剂的使用寿命。该方法工艺简单，成本低，具有原位活性再生能力，具有良好的工业应用前景，对推进水电解制氢技术具有重要意义。

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引用次数: 0

Effects of arginine on the interfacial behavior of proteins 精氨酸对蛋白质界面行为的影响

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-01 Epub Date: 2026-01-21 DOI: 10.1016/j.jcis.2026.139940

Peyman Dastyar , Harsa Mitra , Caitlin V. Wood , Thomas A. Everett , Yu-Jiun Lin , Yu Tian , Arezoo M. Ardekani

Hypothesis: Protein adsorption at fluid-fluid interfaces can induce conformational rearrangements and promote aggregation. Arginine, as an amino acid is known to attenuate protein-protein interactions and lower the viscosity of protein formulations. Given its surface-active properties, we hypothesize that arginine may be effective in limiting aggregation at fluid-fluid interfaces.

Experiments: Interfacial rheology of Etanercept (Enbrel), Immunoglobulin G1 (IgG1), and Bovine Serum Albumin (BSA) was characterized across a range of concentrations, with and without L-arginine Hydrochloride. The interfacial response was examined in both linear and nonlinear regimes. ζ-potential was also measured for selected formulations to evaluate the relationship between electrostatic characteristics and the rheological outcomes.

Findings: Based on both linear and nonlinear interfacial rheology results, arginine generally weakened protein-protein interactions; however, the effect depends on protein identity and concentration. In arginine-containing formulations, Enbrel and BSA displayed only minor variation in interfacial viscoelasticity between 0.01 and 1 mg/mL, particularly during prolonged aging; in contrast, IgG1 showed larger concentration-dependent differences. These results strengthen predictive frameworks for interfacial stability and guide the rational design of protein-amino acid biopharmaceutical formulations.

假设：蛋白质在流体-流体界面的吸附可以诱导构象重排并促进聚集。精氨酸作为一种氨基酸，可以减弱蛋白质之间的相互作用，降低蛋白质配方的粘度。鉴于其表面活性，我们假设精氨酸可能有效地限制了流体-流体界面的聚集。实验：对依那西普（Enbrel）、免疫球蛋白G1 （IgG1）和牛血清白蛋白（BSA）在不同浓度下的界面流变学进行了表征，包括含和不含l -精氨酸盐酸。在线性和非线性两种情况下对界面响应进行了研究。还测量了所选配方的ζ-势，以评估静电特性与流变结果之间的关系。研究发现：基于线性和非线性界面流变学结果，精氨酸通常会减弱蛋白质之间的相互作用；然而，这种效果取决于蛋白质的特性和浓度。在含有精氨酸的配方中，Enbrel和BSA在0.01 ~ 1 mg/mL之间的界面粘弹性变化很小，特别是在长时间老化过程中；相反，IgG1表现出更大的浓度依赖性差异。这些结果加强了界面稳定性的预测框架，并指导蛋白质-氨基酸生物制药配方的合理设计。

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引用次数: 0

Tailoring the structure of MIL-101(Fe) for co-delivery of anti-inflammatory therapeutic agents 调整MIL-101（Fe）的结构，以共同递送抗炎治疗剂

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-01 Epub Date: 2026-01-23 DOI: 10.1016/j.jcis.2026.139968

Aleksandra Galarda , Alicja Warowicka , Aleksander Ejsmont , Joanna Goscianska

Treating inflammation often requires the combined use of multiple agents due to the complexity of biological pathways. Metal–organic frameworks (MOFs), with adjustable structures and high loading capacities, offer a promising route for dual-drug delivery. However, designing MOF-based systems that can simultaneously incorporate and release two distinct anti-inflammatory compounds remains a challenge. In this study, MIL-101(Fe) materials were synthesized under varying temperatures and solvent volumes to tailor their physicochemical properties. Higher synthesis temperatures promoted the formation of more crystalline, microporous structures with well-defined octahedral particles, whereas lower temperatures favored defect-rich, less ordered frameworks. These structural features governed adsorption and enabled controlled release of naproxen sodium and curcumin, selected for complementary action mechanisms. Material synthesized at 110 °C with doubled solvent volumes displayed the most favorable porosity, V_micro/V_total = 0.5, and uniform morphology, achieving high co-adsorption capacity (468 mg/g for naproxen sodium, 160 mg/g for curcumin) along with sustained release (92% and 60% within 24 h at pH 6.8, respectively). Biological evaluation demonstrated that all systems suppressed the synthesis of inflammatory markers, including prostaglandins and IL-6. Notably, the hierarchically porous MIL-101(Fe) synthesized at 110 °C with a higher solvent volume exhibited the strongest COX-1 inhibition (38%), whereas the predominantly mesoporous sample obtained at 110 °C with the standard solvent volume showed greater COX-2 suppression (53%). Low cytotoxicity was observed at 200 μg/mL of the therapeutic agents-loaded carriers, with cell viability remaining over 90%. These findings highlight the potential of MIL-101(Fe) as a tunable carrier for synergistic anti-inflammatory substance delivery.

由于生物途径的复杂性，治疗炎症往往需要多种药物的联合使用。金属有机骨架（MOFs）具有结构可调和高负载能力，是一种很有前景的双药递送途径。然而，设计基于mof的系统能够同时结合和释放两种不同的抗炎化合物仍然是一个挑战。在本研究中，我们在不同的温度和溶剂体积下合成了MIL-101（Fe）材料，以调整其物理化学性质。较高的合成温度有利于形成更结晶的微孔结构，具有明确的八面体颗粒，而较低的合成温度有利于形成富含缺陷的、不太有序的框架。这些结构特征控制了萘普生钠和姜黄素的吸附和控制释放，选择了互补的作用机制。在110℃条件下，双溶剂体积条件下合成的材料孔隙度最佳，Vmicro/Vtotal = 0.5，形貌均匀，共吸附量高（萘普生钠为468 mg/g，姜黄素为160 mg/g），且在pH 6.8条件下24 h内缓释率分别为92%和60%。生物学评价表明，所有系统都抑制炎症标志物的合成，包括前列腺素和IL-6。值得注意的是，在110°C和较高溶剂体积下合成的分层多孔MIL-101（Fe）具有最强的COX-1抑制作用（38%），而在110°C和标准溶剂体积下获得的主要为介孔的样品具有更强的COX-2抑制作用（53%）。在载药浓度为200 μg/mL时，细胞毒性较低，细胞存活率保持在90%以上。这些发现突出了MIL-101（Fe）作为协同抗炎物质递送的可调载体的潜力。

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引用次数: 0

Synergistic enhancement of nitrate-to-ammonia conversion and supercapacitor performance by binuclear copper-modified Keggin-type polyoxometalate complex 双核铜修饰keggin型多金属酸氧配合物协同增强硝酸盐-氨转化和超级电容器性能。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-01 Epub Date: 2026-01-17 DOI: 10.1016/j.jcis.2026.139892

Jiaxing Li, Mengle Yang, Aixiang Tian, Xixian Cao, Jun Ying

The design of electrode materials that combine high efficiency and low cost to effectively reduce environmental pollution and energy consumption represents a core challenge. Herein, a binuclear copper-modified Keggin-type Polyoxometalate (POM) complex based on 1,4-cby ligand (1,4-cby = 1-(4-carboxybenzyl)-4,4′-bipyridine chloride), namely [Cu₂(1,4-cby)₂(1,4-Hcby)₄(H₂O)₂(GeMo₁₂O₄₀)₂]·3H₂O (Cu-GeMo₁₂) is synthesized under hydrothermal conditions by utilizing Keggin POMs, renowned as “electron sponges”, and binuclear copper complex with excellent catalytic activity. Notably, Cu-GeMo₁₂ achieves an outstanding NH₃ yield rate of 14.26 mg h⁻¹ mg_cat⁻¹ and a high Faradaic efficiency of 94.06%, significantly surpassing its mononuclear analogue [Cu(1,4-Hcby)₄]H₃(GeMo₁₂O₄₀)₂ (NH₃ yield rate of 7.73 mg h⁻¹ mg_cat⁻¹ and Faradaic efficiency of 59.83%). Integrated results from in situ Fourier-transform infrared, cyclic voltammetry, and density functional theory calculations reveal that the excellent nitrate-to-ammonia reduction performance of Cu-GeMo₁₂ stems from the continuous electron supply from the POM cluster to the binuclear copper centers, along with the redox-mediating role of the copper sites in promoting the stepwise reduction of nitrogen-containing intermediates. Furthermore, Cu-GeMo₁₂ demonstrates remarkable pseudocapacitive behavior, delivering a high specific capacitance of 1385.09 F·g⁻¹ and retaining 97.27% of its initial capacitance after 5000 cycles. This work provides a novel design strategy for developing POMs functionalized with binuclear metal centers, offering a promising route toward bifunctional materials for applications in electrocatalysis and energy storage.

设计高效、低成本的电极材料，有效降低环境污染和能源消耗是一个核心挑战。本文利用被称为“电子海绵”的Keggin POMs和催化活性优异的双核铜配合物，在水热条件下合成了以1,4-cby配体（1,4-cby = 1-（4-羧基苄基）-4,4′-氯化联吡啶）为基础的双核铜修饰Keggin型多金属氧酸盐（POM）配合物[Cu2(1,4- hcby)2(1,4- hcby)4(H2O)2(GeMo12O40)2]·3H2O （Cu-GeMo12）。值得注意的是，Cu- gemo12的NH3产率为14.26 mg h-1 mgcat-1，法拉第效率为94.06%，显著超过其单核类似物[Cu(1,4- hby)4]H3(GeMo12O40)2 （NH3产率为7.73 mg h-1 mgcat-1，法拉第效率为59.83%）。原位傅里叶变换红外、循环伏安法和密度泛函理论计算的综合结果表明，Cu-GeMo12优异的硝酸盐-氨还原性能源于POM簇连续向双核铜中心提供电子，以及铜位在促进含氮中间体逐步还原中的氧化还原介导作用。此外，Cu-GeMo12表现出了显著的伪电容行为，在5000次循环后，Cu-GeMo12的比电容高达1385.09 F·g-1，保持了97.27%的初始电容。本研究为开发具有双核金属中心功能化的聚甲醛提供了一种新的设计策略，为双功能材料在电催化和储能方面的应用提供了一条有希望的途径。

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引用次数: 0

Plant volatiles-based supramolecular nanoassembly induced by guanidines for sustainable phytopathogen management 胍类化合物诱导植物挥发物超分子纳米组装用于植物病原体可持续管理。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-01 Epub Date: 2026-01-16 DOI: 10.1016/j.jcis.2026.139916

Xiaohong Zhang, Xiaohan Meng, Jianhua Xiao, Yuqi Huang, Weiyao Yan, Gaohua Hu, Qing Guo, Yongqian Liang, Ruyue Han, Jianqiang Li, Gang Tang, Yongsong Cao

Plant volatiles (PVs) are recognized as important mediators of plant interactions with the function of protecting against stress and inducing defense, which presents a potential resource to biopesticides for offering a sustainable and biosafe alternative to conventional agrochemicals. However, PVs exhibit limited bioavailability in practical applications due to the off-target losses caused by high volatility and low thermolability. Here, preselected hydrophobic eugenol (EUG) as a representative molecule and two hydrophilic guanidines (arginine and polyhexamethylene biguanide) as building blocks, two water-based, high-efficiency, and eco-friendly nanosystems (EUG NPs: EA NPs and EP NPs) were developed through self-assembly technology for long-lasting and synergistic phytopathogen management without any hazardous adjuvants. The fabricated EA NPs and EP NPs exhibited high loading rates (48.53% and 42.79%) with small particle sizes of 161 and 157 nm, low polydispersity index values of 0.106 and 0.089, and high ζ-potential values of +38.40 and +58.55 mV. Meanwhile, the resulting EUG NPs displayed improved physicochemical properties, including well-defined nanostructures, low volatilization, and good storage stability, wettability, and adhesion. Importantly, the constructed nanoassemblies could respond to pH changes for long-lasting controlled release of EUG and exhibited high in vitro, in vivo, or postharvest antimicrobial efficacies against Pseudomonas syringae and Botrytis cinerea. Biosafety tests validated that EUG NPs possessed a benign biocompatibility and enabled the promotion of crop seedling growth after the spraying application. These findings illustrate a distinctive perspective for developing PVs as eco-friendly nanopesticides, highlighting a water-based approach for hydrophobic volatile-based biopesticides with improved physicochemical properties and bioavailability.

植物挥发物是植物相互作用的重要介质，具有抗胁迫和诱导防御的功能，为生物农药提供了一种可持续和生物安全的替代传统农用化学品的潜在资源。然而，pv在实际应用中表现出有限的生物利用度，这是由于高挥发性和低耐热性造成的脱靶损失。本研究以预选疏水性丁香酚（EUG）为代表分子，以两种亲水性胍（精氨酸和聚六亚甲基双胍）为基础，通过自组装技术开发了两种水基、高效、环保的纳米系统（EUG NPs: EA NPs和EP NPs），用于长期和协同的植物病原体管理，无需任何有害佐剂。制备的EA NPs和EP NPs具有较高的负载率（48.53%和42.79%），粒径分别为161和157 nm，多分散性指数分别为0.106和0.089，ζ电位分别为+38.40和+58.55 mV。同时，所得EUG NPs的物理化学性质得到了改善，包括纳米结构明确，挥发性低，具有良好的储存稳定性，润湿性和附着力。重要的是，构建的纳米组件可以响应pH变化，长期控制EUG的释放，并在体外、体内或采后对丁香假单胞菌和葡萄孢杆菌具有高的抗菌效果。生物安全性试验证实EUG NPs具有良好的生物相容性，喷施后能促进作物幼苗生长。这些发现为开发pv作为生态友好型纳米农药提供了一个独特的视角，强调了一种基于水的方法来开发具有改善物理化学性质和生物利用度的疏水性挥发性生物农药。

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引用次数: 0

Supramolecular microgels for Pickering emulsion stabilization in the limited coalescence regime: The key role of microgel structure 超分子微凝胶对皮克林乳状液有限聚结稳定性的影响：微凝胶结构的关键作用

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-01 Epub Date: 2026-01-08 DOI: 10.1016/j.jcis.2026.139858

A. Brézault , P. Perrin , P. Garrigue , I. Ly , N. Sanson , V. Schmitt , V. Ravaine

Oil-in-water Pickering emulsions can be stabilized by poly-N-Isopropylacrylamide microgels that adsorb, spread and entangle at the droplets surface. Several studies have tuned the microgels size and deformability to understand the relation between microgel structural parameters, their packing and conformation at the droplet surface and the resulting properties of emulsions. However, both the expected key role of the microgel structure and the mechanism that stops droplets coalescence in the particle-poor regime have never been deciphered. Here, we investigate an unprecedented range of structures, from “ultra” core-shell to more homogeneous ones. First, thanks to Langmuir trough experiments, the free spreading of the microgels at a model interface is proven to be independent of the structure. Second, by contrast, the surface coverage in emulsions

Γ_{emulsion}

, defined as the microgel mass per unit interfacial area, decreases for more core-shell structures. These structures thus stabilize smaller droplets than more homogeneous microgels. Comparing the surface coverage in emulsions to free spreading, it is deduced that the microgel compression at the droplet interface is lower for more core-shell microgels, likely due to their higher ability to make entanglements between adjacent microgels at the interface. Such entanglements counterbalance the overall stresses exerted on the droplets and limit coalescence at lower interfacial compression. Demonstrating the key role played by microgel microstructure in the Limited Coalescence process opens rich perspectives for better controlling emulsion properties.

聚n-异丙基丙烯酰胺微凝胶可以稳定油包水Pickering乳状液，并在液滴表面吸附、扩散和缠结。一些研究调整了微凝胶的尺寸和可变形性，以了解微凝胶结构参数、它们在液滴表面的堆积和构象与乳状液性质之间的关系。然而，预期的微凝胶结构的关键作用和在无粒子状态下阻止液滴聚集的机制从未被破译。在这里，我们研究了前所未有的结构范围，从“超”核-壳到更均匀的结构。首先，通过Langmuir槽实验，证明了微凝胶在模型界面上的自由扩散与结构无关。其次，相比之下，乳液中的表面覆盖率Γemulsion（定义为每单位界面面积的微凝胶质量）随着核-壳结构的增加而降低。因此，这些结构比更均匀的微凝胶稳定更小的液滴。将乳液中的表面覆盖与自由扩散进行比较，可以推断出，核壳微凝胶越多，液滴界面处的微凝胶压缩就越低，这可能是由于它们在界面处相邻微凝胶之间产生缠结的能力越强。这种缠结抵消了施加在液滴上的总应力，并限制了在较低界面压缩时的聚并。揭示微凝胶微观结构在有限聚结过程中的关键作用，为更好地控制乳液性能开辟了丰富的前景。

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引用次数: 0